New optical writing and electrical erasing devices have been successfully fabricated that exploit the photochromism and electrochromism of viologen. In a preliminary study, both the structures of viologen and device were investigated in detail by UV?vis spectra in order to confirm their effects on the optical writing and electrical erasing performances of corresponding devices. For sandwiched, single and complementary devices based on benzyl viologen (BV 2+), only optical writing can be performed, not electrical erasing operations, which indicated these devices cannot realize optical information rewriting. For single and complementary devices based on styrene-functional viologen (V BV 2+) and acrylic-functional viologen (ACV 2+), optical writing and electrical erasing operations can be reversibly performed and optical information rewriting realized. It is clear that single devices based on V BV2+ and ACV2+ possess better performance accompanied with contrast without significant degradation and bleaching times and without significant deterioration over 10 repeated writing/erasing cycles. Furthermore, we put forward possible mechanisms for sandwiched, single and complementary devices based on V BV2+ and ACV2+ for the optical writing and electrical erasing operations. This study provides a new strategy to design optical writing and electrical erasing devices to realize optical information rewriting.